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DOI | 10.1073/pnas.2105628118 |
Atomically dispersed Fe atoms anchored on S and N–codoped carbon for efficient electrochemical denitrification | |
Jiacheng Li; Miao Li; Ning An; Shuo Zhang; Qinan Song; Yilin Yang; Xiang Liu | |
2021-08-17 | |
发表期刊 | Proceedings of the National Academy of Sciences |
出版年 | 2021 |
英文摘要 | Nitrate, a widespread contaminant in natural water, is a threat to ecological safety and human health. Although direct nitrate removal by electrochemical methods is efficient, the development of low-cost electrocatalysts with high reactivity remains challenging. Herein, bifunctional single-atom catalysts (SACs) were prepared with Cu or Fe active centers on an N-doped or S, N–codoped carbon basal plane for N2 or NH4+ production. The maximum nitrate removal capacity was 7,822 mg N ⋅ g−1 Fe, which was the highest among previous studies. A high ammonia Faradic efficiency (78.4%) was achieved at a low potential (−0.57 versus reversible hydrogen electrode), and the nitrogen selectivity was 100% on S-modified Fe SACs. Theoretical and experimental investigations of the S-doping charge-transfer effect revealed that strong metal–support interactions were beneficial for anchoring single atoms and enhancing cyclability. S-doping altered the coordination environment of single-atom centers and created numerous defects with higher conductivity, which played a key role in improving the catalyst activity. Moreover, interactions between defects and single-atom sites improved the catalytic performance. Thus, these findings offer an avenue for high active SAC design. |
领域 | 资源环境 |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/335823 |
专题 | 资源环境科学 |
推荐引用方式 GB/T 7714 | Jiacheng Li,Miao Li,Ning An,等. Atomically dispersed Fe atoms anchored on S and N–codoped carbon for efficient electrochemical denitrification[J]. Proceedings of the National Academy of Sciences,2021. |
APA | Jiacheng Li.,Miao Li.,Ning An.,Shuo Zhang.,Qinan Song.,...&Xiang Liu.(2021).Atomically dispersed Fe atoms anchored on S and N–codoped carbon for efficient electrochemical denitrification.Proceedings of the National Academy of Sciences. |
MLA | Jiacheng Li,et al."Atomically dispersed Fe atoms anchored on S and N–codoped carbon for efficient electrochemical denitrification".Proceedings of the National Academy of Sciences (2021). |
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